US6994936B2 - Nonaqueous electrolyte secondary battery - Google Patents

Nonaqueous electrolyte secondary battery Download PDF

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US6994936B2
US6994936B2 US10/284,237 US28423702A US6994936B2 US 6994936 B2 US6994936 B2 US 6994936B2 US 28423702 A US28423702 A US 28423702A US 6994936 B2 US6994936 B2 US 6994936B2
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nonaqueous electrolyte
secondary battery
electrolyte secondary
battery according
unsaturated bonds
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US20030118914A1 (en
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Sumio Mori
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GS Yuasa International Ltd
GS Yuasa Power Supply Ltd
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Japan Storage Battery Co Ltd
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H01M2300/0028—Organic electrolyte characterised by the solvent
    • H01M2300/0037—Mixture of solvents
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present invention relates to a nonaqueous electrolyte secondary battery wherein the nonaqueous electrolyte contains a sultone compound having unsaturated bonds.
  • a representative battery that can meet such a demand is a lithium secondary battery in which lithium is used as a negative active material.
  • a lithium secondary battery comprises, for example, a negative plate comprising a current collector supporting a carbon material which absorbs and releases lithium ions, a positive plate comprising a current collector supporting a composite lithium oxide such as a lithium-cobalt composite oxide which absorbs and releases lithium ions, and a separator holding an electrolyte solution dissolving such lithium salts as LiClO 4 , LiPF 6 , etc. in an aprotic organic solvent and being interposed between the negative and positive plates to prevent short-circuiting of both plates.
  • the positive and negative plates are formed in thin sheets or foil shapes, and are piled or wound spirally through a intermediary of the separator to form an electric power generating element.
  • the electric power generating element is housed in either a metallic can made of a stainless steel, a nickel plated iron, or lighter aluminum or a battery container made of laminate film, and subsequently an electrolyte is poured into the battery container, which is sealed for fabricating a battery.
  • high-temperature standing characteristics which are particularly important characteristics for such a secondary battery as described above.
  • the high temperature standing characteristics are assessed by measuring the swelling degree and the discharge capacity of the battery after the battery in a charged state has been allowed to stand for a specified duration in an environment where the temperature is 80° C. or above.
  • nonaqueous batteries are more frequently adopted for use in a variety of electronic appliances not only in the atmospheric temperature environment but also in a variety of environments of from low to high temperatures.
  • a cellular telephone left in a sun-heated car makes the nonaqueous electrolyte secondary battery built therein be exposed to a high temperature environment.
  • the characteristics in the high temperature environments of a nonaqueous electrolyte secondary battery becomes important among the characteristics thereof.
  • a lithium secondary battery for use in a cellular telephone is required to be small in the swelling degree thereof when it is allowed to stand at 80° C. for a specified duration.
  • a conventional battery described above is left at a high temperature for a long period of time, the battery sometimes gets swollen owing to the gas generated inside the battery.
  • a battery is demanded to be lighter and thinner, which constitutes a situation in which a battery tends to get more easily swollen.
  • the present invention attempts to obtain an excellent high temperature standing characteristics through suppressing the swelling of a nonaqueous electrolyte secondary battery as represented by a lithium secondary battery, when it is allowed to stand at a high temperature, by making an nonaqueous electrolyte to contain a sultone compound having unsaturated bonds.
  • the vinylene carbonate derivatives be contained in a concentration of 1.0 wt % or below, and/or a cyclic sulfate in a concentration of 2.0 wt % or below in the nonaqueous electrolyte, in addition to the sultone compound having unsaturated bonds, there is prevented the initial discharge capacity degradation occurring when the addition amount of the sultone compound having unsaturated bonds becomes large, so that there can be obtained a nonaqueous electrolyte secondary battery which has excellent high temperature standing characteristics and a large initial discharge capacity.
  • FIG. 1 is a figure illustrating one embodiment of the present invention which shows a sectional view of a prismatic nonaqueous electrolyte secondary battery.
  • the present invention is characterized in that in a nonaqueous electrolyte secondary battery, at least one sultone compound having unsaturated bonds is contained in the nonaqueous electrolyte.
  • the sultone compound having unsaturated bonds is the compound represented by chemical formula (1), where R1 to R4 are independently hydrogen, or the same or different types of alkyl groups, alkoxy groups, halogens, haloalkyl groups, or aryl groups (any group may have unsaturated bonds). Specific examples include 1,3-(1-propene)sultone, 1,3-(1-butene)sultone, 1,3-(2-methyl-1-propene)sultone, 2,4-(2-butene)sultone, etc.
  • the formula represents a compound in which R1 to R4 are independently hydrogen, or the same or different types of alkyl groups, alkoxy groups, halogens, haloalkyl groups, or aryl groups.
  • the high temperature standing characteristics can be improved.
  • SEI solid electrolyte interface
  • the content of the sultone having unsaturated bonds in the nonaqueous electrolyte is preferably 0.2 wt % or above and 2 wt % or below.
  • the content thereof is preferably 0.5 wt % or above and 1 wt % or below.
  • the present invention is also characterized in that the nonaqueous electrolyte contains a vinylene carbonate derivative in 1.0 wt % or below and/or a cyclic sulfate in 2.0 wt % or below, in addition to the sultone compound having unsaturated bonds.
  • the vinylene carbonate derivative and cyclic sulfate are respectively the compounds represented by chemical formula (2) and chemical formula (3), where R5 to R12 are independently hydrogen, or the same or different types of alkyl groups, alkoxy groups, halogens, haloalkyl groups, or aryl groups (any group may contain unsaturated bonds).
  • the formula represents a compound in which R5 to R6 are independently hydrogen, or the same or different types of alkyl groups, alkoxy groups, halogens, haloalkyl groups, or aryl groups.
  • n 0 or 1.
  • the formula represents a compound in which R7 to R12 are independently hydrogen, or the same or different types of alkyl groups, alkoxy groups, halogens, haloalkyl groups, or aryl groups.
  • Examples of the vinylene carbonate derivatives represented by chemical formula (2) include vinylene carbonate, 4,5-dimethylvinylene carbonate, 4,5-diethylvinylene carbonate, 4,5-dipropylvinylene carbonate, 4-ethyl-5-methylvinylene carbonate, 4-ethyl-5-propylvinylene carbonate, etc.
  • Examples of the cyclic sulfate represented by chemical formula (3) include ethylene glycol sulfate, 1,2-propanediol sulfate, 1,2-butanediol sulfate, 1,3-butanediol sulfate, 2,3-butanediol sulfate, phenylethylene glycol sulfate, etc.
  • the degradation of the initial discharge capacity caused by the addition of the sultone compound having unsaturated bonds can be suppressed by making the nonaqueous electrolyte contain the sultone compound having unsaturated bonds, a vinylene carbonate derivative, and/or a cyclic sulfate.
  • the vinylene carbonate derivative or the cyclic sulfate forms an satisfactory SET on the surface of the negative plate, and thereby suppress the formation of the negative plate surface coating film, relatively low in the lithium ion conductivity, by the sultone compound having unsaturated bonds.
  • the content of a vinylene carbonate derivative in the nonaqueous electrolyte is preferably 0.1 wt % or above and 1.0 wt % or below, irrespective of whether a cyclic sulfate is contained or not.
  • the recovering effect can be recognized with the content of the vinylene carbonate as very small as 0.1 wt %.
  • the content of the cyclic sulfate in the nonaqueous electrolyte is preferably 0.1 wt % or above and 2 wt % or below, and it is preferably 0.1 wt % or above and 2.0 wt % or below even when the cyclic sulfate is added together with the vinylene carbonate derivative.
  • the initial discharge capacity decreased with the addition of the sultone compound having unsaturated bonds.
  • the recovering effect can be recognized with the content of the cyclic sulfate as very small as 0.1 wt %. However, when the content of the cyclic sulfate exceeds the above described upper limit, on the contrary, the initial discharge capacity is decreased, and the swelling of the battery becomes remarkable.
  • the nonaqueous electrolyte either an electrolyte solution or a solid electrolyte can be used.
  • an electrolyte solution the following polar solvents and the mixtures thereof can be used: ethylene carbonate, prolpylene carbonate, dimethyl carbonate, ethyl methyl carbonate, diethyl carbonate, ⁇ -butyrolactone, sulfolane, dimethyl sulfoxide, acetonitrile, dimethyl formamide, dimethyl acetamide, 1,2-dimethoxyethane, 1,2-diethoxyethane, tetrahydrofuran, 2-methyltetrahydorfuran, dioxolane, methyl acetate, etc.
  • the solvent to be used for the electrolyte solution contains ethylene carbonate, among these solvents, in order to improve the discharge characteristics and life characteristics of a battery.
  • the electrolyte salts to be dissolved in the solvent of the electrolyte solution are the following salts and the mixtures thereof: LiPF 6 , LiClO 4 , LiBF 4 , LiAsF 6 , LiCF 3 CO 2 , LiCF 3 (CF 3 ) 3 , LiCF 3 (C 2 F 5 ) 3 , LiCF 3 SO 3 , LiN(SO 2 CF 3 ) 2 , LiN(SO 2 CF 2 CF 3 ) 2 , LiN(COCF 3 ) 2 , LiN(COCF 2 CF 3 ) 2 , and LiPF 3 (CF 2 CF 3 ) 3 .
  • the electrolyte salts to be added to the electrolyte solution partially contain LiPF 6 and LiBF 4 .
  • the composite oxides represented by the composition formulas Li x MO 2 , Li y M 2 O 4 , and Na x MO 2 (M stands for one or more than one types of transition metals, 0 ⁇ x ⁇ 1, 0 ⁇ y ⁇ 2) and a metal chalcogenide or a metal oxide which has either a tunnel structure or a layer structure.
  • Specific examples include LiCoO 2 , LiCo x Ni 1-x O 2 , LiMn 2 O 4 , Li 2 Mn 2 O 4 , MnO 2 , FeO 2 , V 2 O 5 , V 6 O 13 , TiO 2 , TiS 2 , etc.
  • a conducting polymer such as polyaniline can be used as any mixture of the above described active materials, irrespective of whether inorganic or organic, may be used.
  • a negative active material there may be used the alloys of Li with Al, Si, Pb, Sn, Zn, Cd, etc., metal oxides such as LiFe 2 O 3 , WO 2 , MoO 2 , SiO, and CuO, carbon materials such as graphite, and carbon, lithiumnitrides such as Li 5 (Li 3 N), ormetalliclithium, orthemixtures thereof.
  • metal oxides such as LiFe 2 O 3 , WO 2 , MoO 2 , SiO, and CuO
  • carbon materials such as graphite, and carbon
  • lithiumnitrides such as Li 5 (Li 3 N)
  • woven cloth, nonwoven cloth, microporous synthetic resin film, etc. there can be used woven cloth, nonwoven cloth, microporous synthetic resin film, etc., and particularly microporous synthetic resin film can be used suitably.
  • the microporous films made of polyethylene and polypropylene, and the polyolefin-based microporous films such as the microporous films derived from combination thereof are used suitably in view of the film thickness, film strength, and film resistance, etc.
  • Solid electrolytes such as polymer solid electrolytes, which work simultaneously as separators, can be used.
  • a porous polymer solid electrolyte film is used as the polymer solid electrolyte, and the solid electrolyte film can be made to contain an electrolyte solution.
  • the electrolyte solution composing the gel and the electrolyte solution contained in the pores may be different from each other.
  • the electrolyte solution can contain the sultone compounds having unsaturated bonds, vinylene carbonate derivatives, or cyclic sulfates of the present invention.
  • synthetic resin microporous films and polymer solid electrolytes etc. may be used in combination.
  • the present invention can be applied to such a various shapes of nonaqueous electrolyte secondary batteries as prismatic, elliptical, coin-shaped, button-shaped, sheet-shaped batteries, etc.
  • the present invention intends to suppress the swelling of a battery when the battery is allowed to stand at a high temperature, and accordingly the present invention provides remarkable effects when battery cases are weak in mechanical strength, and in particular, battery cases made of aluminum or aluminum laminate are used.
  • FIG. 1 is a figure outlining a sectional view of a prismatic nonaqueous electrolyte secondary battery of the present embodiment.
  • the prismatic nonaqueous electrolyte secondary battery 1 comprises a group of flat and wound plates 2 and a nonaqueous electrolyte, both housed in a battery case 6 .
  • the dimension of the battery is 30 mm in width ⁇ 48 mm in height ⁇ 4 mm in thickness.
  • the group of plates is fabricated by winding together spirally a positive plate 3 made of an aluminum current collector coated with a positive active material and a negative plate 4 made of a copper current collector coated with a negative active material, through a intermediary of the separator 5 .
  • a battery cap 7 equipped with a safety valve 8 is fixed to a battery case 6 by laser welding, a negative plate terminal 9 is connected to a negative plate 4 via a lead wire for the negative plate 11 , and a positive plate 3 is connected to the battery cap via a lead wire for the positive plate 10 .
  • the positive plate was formed as follows: A positive composite was prepared by mixing polyfluorovinylidene (8 wt %) as a binder, acetylene black (5 wt %) as a conducting material, and a lithium cobalt composite oxide (87 wt %) as a positive active material. N-methylpyrrolidone was added to the positive composite to prepare a pasty positive composite. The pasty positive composite was applied onto both sides of an aluminum foil current collector of 20 ⁇ m in thickness and the coated layers were dried.
  • a negative plate was formed as follows: A pasty composite was prepared from graphite (95 wt %), carboxymethyl cellulose (2 wt %), styrene-butadiene rubber (3 wt %), and an appropriate amount of water. The pasty composite was applied onto both sides of a copper foil current collector of 15 ⁇ m in thickness, and the coated layers were dried.
  • a sheet of polyethylene microporous film was used as a separator.
  • the nonaqueous electrolytes were prepared as follows: The lithium salt LiPF 6 was dissolved in a concentration of 1 mol/l in a mixed solvent of ethylene carbonate and ethyl methyl carbonate (4:6 in volume ratio). To this solution as base, 1,3-(1-propene) sultone represented by chemical formula (4) was added in the range from 0.2 to 2.0 wt % in relation to the total amount of the electrolyte, vinylene carbonate represented by chemical formula (5) was added in the range from 0.1 to 2.0 wt %, and ethylene glycol sulfate represented by chemical formula (6) was added in the range from 0.1 to 4.0 wt %, thus obtaining various electrolytes.
  • 1,3-(1-propene) sultone represented by chemical formula (4) was added in the range from 0.2 to 2.0 wt % in relation to the total amount of the electrolyte
  • vinylene carbonate represented by chemical formula (5) was added in the range from 0.1 to 2.0
  • Table 1 collects the contents of 1,3-(1-propene)sultone, vinylene carbonate, and ethylene glycol sulfate in the nonaqueous electrolytes used in the batteries of Examples 1 to 41 and Comparative Examples 1 to 3.
  • Example 1 0.2 No No 608 4.68
  • Example 2 0.2 0.1 No 610 4.67
  • Example 3 0.2 0.5 No 614 4.69
  • Example 4 0.2 1.0 No 615 4.68
  • Example 5 0.2 2.0 No 615 4.98
  • Example 6 0.2 No 0.1 612 4.65
  • Example 7 0.2 No 0.5 614 4.63
  • Example 8 0.2 No 1.0 613 4.65
  • Example 9 0.2 No 2.0 612 4.67
  • Example 10 0.2 No 4.0 611 4.94
  • Example 11 0.5 No No 606 4.51
  • Example 12 0.5 0.1 No 608 4.50
  • Example 13 0.5 0.5 No 612 4.49
  • Example 14 0.5 1.0 No 614 4.51
  • Example 15 0.5 2.0 No 615 4.91
  • Example 16 0.5 No 0.1 610 4.48
  • Example 17 0.5 No 0.5 612 4.47
  • Example 18 0.5 No 1.0 611 4.
  • the initial capacity is the discharge capacity measured as follows: a battery is charged for 2.5 hours under the constant current-constant voltage charging conditions wherein the charge current is 600 mA and the charge voltage is 4.20 V, and subsequently the discharge capacity is measured under the discharge conditions where the discharge current is 600 mA and the cut-off voltage is 2.75 V.
  • the battery thickness measurement after being allowed to stand at a high temperature is the battery thickness measured as follows: a battery which has been subjected to the initial capacity examination is charged for 2.5 hours under the constant current-constant voltage charging conditions where the current is 600 mA and the voltage is 4.20 V; subsequently the battery is allowed to stand at 80° C. for 50 hours; and then the battery is cooled down to room temperature and the battery thickness is measured.
  • Table 1 collects the test and measurement results for the batteries of Examples and Comparative Examples, together with the additive contents. For each test and measurement, the listed value is the average value over the values obtained for ten batteries.
  • Example 10 Example 20
  • Example 30 Example 40
  • the battery thickness after being allowed to stand at a high temperature becomes larger, despite the addition of 1,3-(1-propene)sultone.
  • the battery swelling after being allowed to stand at a high temperature is able to be made small.
  • the addition amount of 1,3-(1-propene)sultone is large, the initial discharge capacity is decreased, but the initial discharge capacity degradation is able to be suppressed by the addition of vinylene carbonate in 1.0 wt % or below in addition to 1,3-(1-propene) sultone.
  • the initial discharge capacity degradation is also able to be suppressed by the addition of ethylene glycol sulfate in 2.0 wt % or below in addition to 1,3-(1-propene)sulfone.
  • Example 41 As can be seen from the results of Example 41, it has been found that there can also be obtained a battery in which the battery swelling caused by being allowed to stand at a high temperature is small and the discharge capacity is large, when vinylene carbonate (1.0 wt %) and ethylene glycol sulfate (2.0 wt %) are added in addition to 1,3-(1-propene)sultone (2.0 wt %).
  • the solvents used are ethylene carbonate and ethyl methyl carbonate. Results similar to those in Example 41 can also be obtained when dimethyl carbonate, diethyl carbonate, ⁇ -butyrolactone, and propylene carbonate are used in place of ethyl methyl carbonate, or when the concentration of LiPF 6 as solute is varied or the type of the solute is varied.
  • the solvent and solute composing the nonaqueous electrolyte should not be limited to those combinations which are used in Examples.
  • Examples include the examples wherein vinylene carbonate and/or ethylene glycol sulfate is added in addition to 1,3-(1-propene)sultone. Effects similar to those obtained with vinylene carbonate and/or ethylene glycol sulfate can be obtained when in place of vinylene carbonate, there are used the vinylene carbonate derivatives represented by chemical formula (2), such as 4,5-dimethylvinylene carbonate, 4,5-diethylvinylene carbonate, 4,5-dipropylvinylene carbonate, 4-ethyl-5-methylvinylene carbonate, 4-ethyl-5-propylvinylene carbonate.
  • chemical formula (2) such as 4,5-dimethylvinylene carbonate, 4,5-diethylvinylene carbonate, 4,5-dipropylvinylene carbonate, 4-ethyl-5-methylvinylene carbonate, 4-ethyl-5-propylvinylene carbonate.
  • cyclic sulfates represented by chemical formula (3) such as 1,2-propanediol sulfate, 1,2-butanediolo sulfate, 1,3-butanediol sulfate, 2,3-butanediol sulfate, and phenylethylene glycol sulfate.
  • substituent groups in the sultone compounds having unsaturated bonds (chemical formula (1)), the vinylene carbonate derivatives (chemical formula (2)), and the cyclic sulfates (chemical formula (3)) are not restricted to hydrogen, but may be alkyl, alkoxy, halogen, haloalkyl, or aryl (unsaturated bonds may be contained in any group). It may be noted that the number of moles of a compound having a larger molecular weight becomes smaller for a certain addition amount. In order to prevent the cost rise and the adverse effects on the battery characteristics, etc., substituents of lower molecular weights are desirable.
  • the positive and negative active materials are not limited to the combinations mentioned in the above descriptions of Examples, but the various active materials mentioned in the above descriptions of Embodiments can be used.
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